TWI274771B - Resin composition, prepreg and laminate using the same - Google Patents

Resin composition, prepreg and laminate using the same Download PDF

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Publication number
TWI274771B
TWI274771B TW93130201A TW93130201A TWI274771B TW I274771 B TWI274771 B TW I274771B TW 93130201 A TW93130201 A TW 93130201A TW 93130201 A TW93130201 A TW 93130201A TW I274771 B TWI274771 B TW I274771B
Authority
TW
Taiwan
Prior art keywords
resin
mass
resin composition
compound
content
Prior art date
Application number
TW93130201A
Other languages
Chinese (zh)
Other versions
TW200519162A (en
Inventor
Kousuke Hirota
Koutarou Asahina
Kenji Shima
Hitoshi Sakuraba
Takashi Iiyama
Original Assignee
Mitsui Chemicals Inc
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Publication date
Application filed by Mitsui Chemicals Inc filed Critical Mitsui Chemicals Inc
Publication of TW200519162A publication Critical patent/TW200519162A/en
Application granted granted Critical
Publication of TWI274771B publication Critical patent/TWI274771B/en

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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L79/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen with or without oxygen or carbon only, not provided for in groups C08L61/00 - C08L77/00
    • C08L79/04—Polycondensates having nitrogen-containing heterocyclic rings in the main chain; Polyhydrazides; Polyamide acids or similar polyimide precursors
    • C08L79/08—Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
    • B32B5/26—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer another layer next to it also being fibrous or filamentary
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L61/00—Compositions of condensation polymers of aldehydes or ketones; Compositions of derivatives of such polymers
    • C08L61/04—Condensation polymers of aldehydes or ketones with phenols only
    • C08L61/06—Condensation polymers of aldehydes or ketones with phenols only of aldehydes with phenols
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2260/00—Layered product comprising an impregnated, embedded, or bonded layer wherein the layer comprises an impregnation, embedding, or binder material
    • B32B2260/04—Impregnation, embedding, or binder material
    • B32B2260/046—Synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2305/00—Condition, form or state of the layers or laminate
    • B32B2305/07—Parts immersed or impregnated in a matrix
    • B32B2305/076—Prepregs
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/30—Properties of the layers or laminate having particular thermal properties
    • B32B2307/306—Resistant to heat
    • B32B2307/3065—Flame resistant or retardant, fire resistant or retardant
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/70—Other properties
    • B32B2307/724—Permeability to gases, adsorption
    • B32B2307/7242—Non-permeable
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2457/00—Electrical equipment
    • B32B2457/08—PCBs, i.e. printed circuit boards
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2201/00—Properties
    • C08L2201/02—Flame or fire retardant/resistant
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00—Polymer mixtures characterised by other features
    • C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2666/00—Composition of polymers characterized by a further compound in the blend, being organic macromolecular compounds, natural resins, waxes or and bituminous materials, non-macromolecular organic substances, inorganic substances or characterized by their function in the composition
    • C08L2666/02—Organic macromolecular compounds, natural resins, waxes or and bituminous materials
    • C08L2666/14—Macromolecular compounds according to C08L59/00 - C08L87/00; Derivatives thereof
    • C08L2666/22—Macromolecular compounds not provided for in C08L2666/16 - C08L2666/20
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/31504—Composite [nonstructural laminate]
    • Y10T428/31511—Of epoxy ether
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/31504—Composite [nonstructural laminate]
    • Y10T428/31511—Of epoxy ether
    • Y10T428/31515—As intermediate layer

Landscapes

  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Materials Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Reinforced Plastic Materials (AREA)
  • Epoxy Resins (AREA)
  • Laminated Bodies (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

A laminate is provided. The laminate doesn't contain halogen and the laminate, even with a thickness of no more than 0.2 mm, is highly fire-resistant, and has the moisture-enduring, heat-resisting property for hygroscopic solder. In the resin composition, a prepreg and a laminate using the same, the resin composition includes (A) a compound containing no less than two maleimide groups; (B) the phenolic resin; (C) epoxy resin. The present invention is characterized in that at least one of (B) and (C) includes a compound containing naphthalene ring. The total mass of naphthalene ring calculated from OH-equivalent of (B) and epoxy-equivalent of (C) is no less than 20% in the total mass of components (A)+(B)+(C), and the sum of a content of component (A) in the total mass of components (A)+(B)+(C) and a content of naphthalene ring is no less than 65%.

Description

1274771 14873pif.doc 九、發明說明： 【發明所屬之技術領域】 本發明關於一種在電子·電氣部件、印刷電路板、半 導體基板、1C封裝材料等電子材料領域內使用的樹脂組成 物及其用途，更詳細地說，關於一種樹脂組成物、使用該 樹脂組成物的預浸體(prepreg)及積層板，所述樹脂組成物 不含有含鹵素阻燃劑、含磷阻燃劑，特別適用於要求高耐 熱性的印刷電路板、半導體基板，並且具有優良的吸濕耐 熱性、耐濕性。 【先前技術】 在電子材料領域內，爲了確保對火災的安全性，而要求 具有阻燃性。對於用於印刷電路板、半導體基板的積層板 材料而言，其代表性標準爲美國安全檢測實驗室公司 (Underwriters Laboratories lnc )的 UL94 標準，要求在垂直 燃燒試驗中，優選在V - 1、更優選在v一 〇條件下達到合 格標準。目前，爲了使該領域內使用的樹脂均在該條件下 達到合格標準，而使其含有含溴化合物等含鹵化合物作爲 阻燃劑。所述含鹵化合物具有高阻燃性，但是，例如芳香 族溴化物不僅經熱分解產生具有腐蝕性的溴、溴化氫，而 且在氧氣存在下，可能形成毒性高的化合物（參見西澤仁， “鹵系阻燃劑”，聚合物的阻燃化，大成社，pp 69〜 79(1992))。 基於上述原因，開始硏究開發不含有鹵素化合物的材 料，即所謂“無鹵”材料（例如，參見特開2〇〇3 一 23 1762 1274771 14873pif.doc 號公報等）。其中，作爲代替含鹵化合物的阻燃劑，以紅磷 等含磷化合物爲中心進行了硏究。但是，含磷阻燃劑在燃 燒時可能產生磷化氫等有毒磷化合物，而且使用代表性的 磷酸酯作爲含磷化合物阻燃劑時，存在顯著損害組成物耐 濕性的缺點。 另一方面，作爲其他阻燃劑，已知有金屬氫氧化物，例 如已知利用氫氧化鋁在加熱時放出結晶水的下述反應，可 以發揮作爲阻燃劑的效果。 2A1(0H)3->A12034- 3H20 但是’單獨使用氫氧化鋁等金屬氫氧化物作爲阻燃劑 時’爲了得到所要求的阻燃性能，必須添加大量的該金屬 氫氧化物。在使用常見的環氧樹脂、添加氫氧化銘作爲阻 燃劑製成積層板的情況下，爲了達到UL94標準的V— 0級 別，氫氧化鋁的必需添加量爲樹脂組成物的70wt%〜75wt %左右，即使使用具有不易燃燒骨架的樹脂，也必須添加 50wt%左右的氫氧化鋁（參見木內幸浩，位地正年，電子封 裝學會誌，5(2)ρρ·159〜165(2003))。在氫氧化鋁的添加量 多的情況下，樹脂組成物及由該樹脂形成的積層板的性 能、特別是耐濕性及吸濕後的耐熱性（銲料耐熱性）顯著降低 (參見特開2001 - 226465號公報）。在將積層板作爲半導體 用基板等使用的情況下，耐濕性或吸濕後的耐熱性對封裝 時的可靠性有較大影響，因此要求加以改善。 另外，目前在評價積層板的阻燃性時，多採用厚度爲 1.6mm等的積層板進行評價。但是，隨著近年來電子機器 1274771 14873pif.doc 的輕薄短小化’要求作爲半導體基板使用的積層板的厚度 爲0.5mm 1 〇 5mm以下’優選爲〇 2mm或0.2mm以下。 &度越薄’燃燒時越容易與氧氣接觸，也越容易燃燒，因 此通常需要較多的阻燃劑。從而，爲了得到滿足較薄積層 板的阻燃㈣求、並頭有充分麵濕性、賴後的銲料 耐熱性的積層板材料，需要一種阻燃性高的樹脂組成。 作爲上述阻燃性高的樹脂，本發明人提出了含有特定馬 來醯亞胺基的樹脂組成（參見特開2003 - 119348號公報， 特開2003 - 147170號公報）。但是，即使採用上述樹脂組 成’也難以獲得足以耐受使用〇.2mni或〇.2mill以下薄板進 行的嚴格阻燃性試驗的阻燃性。另一方面，已知在爲了提 高在基板材料所要求的吸濕條件下的耐熱性而使用含有萘 環的特定環氧樹脂時，能夠得到充分的耐熱性（參見特開 2003 - 335925號公報）。但是，由於耐熱性和阻燃性未必一 致’因此難以得到同時具有充分的耐熱性和阻燃性的樹脂 組成。 【發明內容】 本發明的目的爲提供一種樹脂組成物以及積層板，所述 樹脂組成物不含鹵素，並且在作爲基板使用時，即使厚度 爲0.5 mm或0.5mm以下，也能夠具有充分的阻燃性，而且 具有充分的耐濕性和吸濕銲料耐熱性。 ， 爲了解決上述問題，本發明人進行了深入硏究，結果發 現了一種含有含特定馬來醯亞胺基的化合物、酚醛樹脂、 環氧樹脂的樹脂組成物，酚醛樹脂和環氧樹脂中的至少一 12747¾ 73pif.doc 方包含具有萘環的化合物，該樹脂中所含萘環的質量總和 爲特定比例或該比例以上，並且含有馬來醯亞胺基的化合 物的含有率與樹脂中所含萘環的含有率總和在特定範圍內 時，能夠得到具有特別優良的阻燃性、耐濕熱性的組成物， 從而完成本發明。 即，本發明關於以下內容。 1) 一種樹脂組成物，含有： (A) 含有至少2個或2個以上馬來醯亞胺基的化合物， (B) 酚醛樹脂， (C) 環氧樹脂， 其特徵爲，（B)或（C)中至少一方包含具有萘環的化合 物，使用（B)和（C)各自的0H當量、環氧當量計算的萘環質 量總和相對於(A)+(B)+(C)成分質量總和爲20質量％或 20質量％以上，且（A)成分相對於(A) + (B) + (C)成分總質量 的含有率與該萘環的含有率總和爲65質量％或65質量％ 以上；優選爲： 2) 如1)所述的樹脂組成物，其中，（A)含有至少2個或 2個以上馬來醯亞胺基的化合物的含量相對於(A)+ (B) + (C)成分質量總和，以馬來醯亞胺環中包含的氮原子含量計 爲3.5質量％或3.5質量％以上；更優選爲： 3) 如1)所述的樹脂組成物，其中，該組成物中還含有金 屬氫氧化物；以及 4) 一種預浸體，其特徵爲，所述預浸體是藉由使1)所述 的樹脂組成物含浸在基材中而得到的；以及， 9 1274771 14873pif.doc 5) —種積層板，其特徵爲，所述積層板是藉由將由〗張 或幾張4)所述的預浸體積層而成的材料加熱固化而得到 的；另外， 6) —種積層板，其特徵爲，該積層板含有由1}所述的樹 脂組成物得到的樹脂作爲絕緣層。 由於本發明的樹脂組成物具有高阻燃性，因此即使形成 0.5mm或〇.5mm以下的薄積層板，也能夠得到充分的阻燃 性。另外，由於樹脂組成物的阻燃性高，因此可以不添加/ 或與通常情況相比僅添加少量金屬氫氧化物等能夠使吸濕 特性劣化的阻燃劑，其結果爲使樹脂組成物、以及由此形 成的積層板具有高耐濕性、吸濕耐熱性。 【實施方式】 下面，詳細說明本發明。 本發明的樹脂組成物包含(A)含有至少2個或2個以上 馬來醯亞胺基的化合物，（B)酚醛樹脂，（C)環氧樹脂。 首先，就構成本發明樹脂組成物的各成分進行說明。 (A)含有至少2個或2個以上馬來醯亞胺基的化合物 本發明中使用的含有至少2個或2個以上馬來醯亞胺基 的化合物只要是含有至少2個或2個以上馬來醯亞胺基的 化合物即可，沒有特別限定，優選下述通式（1)表示的化合 物。 (々士 R1⑴ 〇 (式中，R!表示m價的有機基；m爲2或2以上的整數， 1274771 14873pif.doc 優選爲2〜10 ;作爲R:表示的有機基，優選從由下述通式 (2 — 1)〜（2 — 3)組成的族群中選擇的基。）[Technical Field] The present invention relates to a resin composition used in the field of electronic materials such as electronic/electrical components, printed circuit boards, semiconductor substrates, and 1C packaging materials, and uses thereof. More specifically, the present invention relates to a resin composition, a prepreg using the resin composition, and a laminate, which does not contain a halogen-containing flame retardant or a phosphorus-containing flame retardant, and is particularly suitable for use in a resin composition. A highly heat-resistant printed circuit board or a semiconductor substrate, and has excellent moisture absorption and heat resistance and moisture resistance. [Prior Art] In the field of electronic materials, flame retardancy is required in order to ensure safety against fire. For laminated board materials used in printed circuit boards and semiconductor substrates, the representative standard is the UL94 standard of Underwriters Laboratories lnc, which is required to be in the vertical burning test, preferably at V-1. It is preferred to meet the eligibility criteria under v-〇 conditions. At present, in order to make the resins used in the field meet the qualification standards under such conditions, they contain a halogen-containing compound such as a bromine-containing compound as a flame retardant. The halogen-containing compound has high flame retardancy, but, for example, the aromatic bromide not only thermally decomposes to produce corrosive bromine or hydrogen bromide, but also may form a highly toxic compound in the presence of oxygen (see Nishizawa, "Halogen-based flame retardants", flame retardant of polymers, Dachengshe, pp 69~79 (1992)). For the above reasons, development of a material which does not contain a halogen compound, that is, a so-called "halogen-free" material (for example, see Japanese Patent Laid-Open Publication No. Hei. No. Hei. Among them, as a flame retardant instead of a halogen-containing compound, research has been focused on a phosphorus-containing compound such as red phosphorus. However, a phosphorus-containing flame retardant may generate a toxic phosphorus compound such as phosphine when burned, and when a representative phosphate ester is used as a phosphorus-containing compound flame retardant, there is a disadvantage that the moisture resistance of the composition is remarkably impaired. On the other hand, as the other flame retardant, a metal hydroxide is known. For example, the following reaction using aluminum hydroxide to release crystal water upon heating can be used, and the effect as a flame retardant can be exhibited. 2A1(0H)3->A12034- 3H20 However, when a metal hydroxide such as aluminum hydroxide is used alone as a flame retardant, it is necessary to add a large amount of the metal hydroxide in order to obtain desired flame retardancy. In the case of using a common epoxy resin and adding a hydroxide as a flame retardant to form a laminate, in order to achieve the V-0 level of the UL94 standard, the necessary addition amount of aluminum hydroxide is 70 wt% to 75 wt of the resin composition. About 5% or so, even if a resin having a non-flammable skeleton is used, it is necessary to add about 50% by weight of aluminum hydroxide (see Yuki Koike, the place of the year, Electronic Packaging Society, 5(2) ρρ·159~165 (2003) ). When the amount of addition of aluminum hydroxide is large, the properties of the resin composition and the laminate formed of the resin, particularly the moisture resistance and the heat resistance after moisture absorption (solder heat resistance) are remarkably lowered (see JP-2001). - 226465). When the laminate is used as a substrate for a semiconductor or the like, the moisture resistance or the heat resistance after moisture absorption greatly affects the reliability at the time of packaging, and therefore it is required to be improved. Further, at the time of evaluating the flame retardancy of the laminated board, a laminate having a thickness of 1.6 mm or the like is often used for evaluation. However, with the recent reduction in the thickness and thickness of the electronic device 1274771 14873pif.doc, the thickness of the laminated board used as the semiconductor substrate is required to be 0.5 mm 1 〇 5 mm or less', preferably 〇 2 mm or less. The thinner the & degree, the easier it is to contact with oxygen when burning, and the easier it is to burn, so more flame retardant is usually required. Therefore, in order to obtain a laminated board material which satisfies the flame retardancy (fourth) of the thin laminated board and has sufficient surface wettability and solder heat resistance, a resin composition having high flame retardancy is required. The present inventors have proposed a resin composition containing a specific maleimide group as a resin having a high flame retardancy (see JP-A-2003-119348, JP-A-2003-147170). However, even with the above resin composition ', it is difficult to obtain flame retardancy sufficient to withstand the strict flame retardancy test conducted using a sheet of 〇.2mni or 〇.2mill or less. On the other hand, it is known that when a specific epoxy resin containing a naphthalene ring is used in order to improve the heat resistance under the moisture absorption conditions required for the substrate material, sufficient heat resistance can be obtained (see JP-A-2003-335925). . However, since heat resistance and flame retardancy are not necessarily uniform, it is difficult to obtain a resin composition having sufficient heat resistance and flame retardancy at the same time. SUMMARY OF THE INVENTION An object of the present invention is to provide a resin composition containing no halogen, and which can have sufficient resistance even when the thickness is 0.5 mm or less when used as a substrate. It is flammable and has sufficient moisture resistance and moisture resistance of solder. In order to solve the above problems, the inventors conducted intensive studies and found a resin composition containing a specific maleidinium group-containing compound, a phenol resin, an epoxy resin, a phenol resin, and an epoxy resin. At least one 127,473⁄4 73 pif.doc side comprises a compound having a naphthalene ring, the total mass of the naphthalene ring contained in the resin is a specific ratio or more, and the content of the compound containing a maleimine group is contained in the resin. When the total content of the naphthalene ring is within a specific range, a composition having particularly excellent flame retardancy and moist heat resistance can be obtained, and the present invention has been completed. That is, the present invention relates to the following. 1) A resin composition comprising: (A) a compound containing at least 2 or more maleimine groups, (B) a phenol resin, (C) an epoxy resin, characterized by (B) or At least one of (C) includes a compound having a naphthalene ring, and the total mass of the naphthalene ring calculated from the respective 0H equivalents and epoxy equivalents of (B) and (C) is relative to the mass of the (A)+(B)+(C) component. The sum is 20% by mass or more, and the total content of the component (A) relative to the total mass of the (A) + (B) + (C) component and the total content of the naphthalene ring are 65 mass% or 65 mass. The resin composition according to 1), wherein (A) the content of the compound containing at least two or more maleimine groups is relative to (A) + (B) The sum of the mass of the component (C) is 3.5% by mass or more, and more preferably: 3) The resin composition as described in 1), wherein, The composition further contains a metal hydroxide; and 4) a prepreg characterized in that the prepreg is impregnated into the substrate by the resin composition of 1). And 9 1274771 14873pif.doc 5) - a laminated board characterized in that the laminated board is heat-cured by a material obtained by laminating a prepreg layer of the sheet or sheets 4) Further, 6) is a laminated board characterized in that the laminated board contains a resin obtained from the resin composition described in 1} as an insulating layer. Since the resin composition of the present invention has high flame retardancy, sufficient flame retardancy can be obtained even if a thin laminate having a thickness of 0.5 mm or less is formed. In addition, since the flame retardancy of the resin composition is high, it is possible to add a small amount of a metal hydroxide or the like, which is capable of deteriorating hygroscopic properties, without adding/or adding a resin composition, and as a result, a resin composition, And the laminate formed thereby has high moisture resistance, moisture absorption and heat resistance. [Embodiment] Hereinafter, the present invention will be described in detail. The resin composition of the present invention comprises (A) a compound containing at least two or more maleimine groups, (B) a phenol resin, and (C) an epoxy resin. First, each component constituting the resin composition of the present invention will be described. (A) A compound containing at least two or more maleimine groups. The compound containing at least two or more maleimine groups used in the present invention contains at least two or more. The compound of the maleimine group is not particularly limited, and a compound represented by the following formula (1) is preferred. (Gentleman R1(1) 〇 (wherein R! represents an m-valent organic group; m is an integer of 2 or more, 1274771 14873pif.doc is preferably 2 to 10; and as an organic group represented by R: preferably from the following a group selected from the group consisting of (2 - 1) to (2 - 3).)

(2-3) (式中，X可以彼此相同，也可以不同，表示—ch2—、 一 C(CH3)2—、一 C(C2H5)2—、一 c〇一、一〇一、一（單鍵）、 —S —或—S〇2—。Y可以彼此相冋’也可以不问’表不一 CH3、— CH2CH3、或氫原子。） 作爲本發明中可以使用的含有至少2個或2個以上馬來 醯亞胺基的化合物，具體而言，例如可以舉出N，N’-（1，3 一亞苯基）雙馬來醯亞胺、N，N’一 [1，3 -（2 —甲基亞苯基）] 雙馬來醯亞胺、N，N’-（1，4 一亞苯基）雙馬來醯亞胺、雙（4 -馬來醯亞胺基苯基）甲烷、雙（3 -甲基-4-馬來醯亞胺基 苯基）甲烷、雙（4-馬來醯亞胺基苯基）醚、雙（4-馬來醯亞 胺基苯基）楓、雙（4-馬來醯亞胺基苯基）硫醚、雙（4-馬來 醯亞胺基苯基）酮、1，4-雙（馬來醯亞胺基甲基）苯、1，3-雙 (3-馬來醯亞胺基苯氧基）苯、雙[4 -（4-馬來醯亞胺基苯 氧基）苯基]甲烷、U—雙[4 一（3—馬來醯亞胺基苯氧基）苯 基]乙烷、U-雙[4 一（4 一馬來醯亞胺基苯氧基）苯基]乙 烷、1，2-雙[4 一（3—馬來醯亞胺基苯氧基）苯基]乙烷、1，2 一雙[4 一（4 一馬來醯亞胺基苯氧基）苯基]乙烷等。 1274771 另外，作爲本發明中使用的含有至少2個或2個以上馬 來醯亞胺基的化合物，還可以舉出下述通式（3)表示的含馬 來醯亞胺基的化合物以及下述通式（4)表示的含馬來醯亞胺 基的化合物等。上述含馬來醯亞胺基的化合物(A)可以單獨 使用，可以將2種或2種以上組合使用。(2-3) (wherein, X may be the same as each other, or may be different, indicating -ch2 -, a C(CH3)2 -, a C(C2H5)2 -, a c〇1, a 〇一, a ( A single bond), -S - or -S〇2 -. Y may be mutually exclusive 'may also be 'not asked' for CH3, -CH2CH3, or a hydrogen atom.) As the present invention, it may contain at least 2 or Examples of the compound of two or more maleic imine groups include, for example, N,N'-(1,3-phenylene) bismaleimide, N,N'-[1,3 -(2-methylphenylene)] bismaleimide, N,N'-(1,4-phenylene) bismaleimide, bis(4-maleimidobenzene) Methane, bis(3-methyl-4-maleimidophenyl)methane, bis(4-maleimidophenyl)ether, bis(4-maleimidobenzene) Base), bis(4-maleimidophenyl) sulfide, bis(4-maleimidophenyl)one, 1,4-bis(maleimidomethyl) Benzene, 1,3-bis(3-maleimidophenoxy)benzene, bis[4-(4-maleimidophenoxy)phenyl]methane, U- Bis[4-(3-maleimidophenoxy)phenyl]ethane, U-bis[4-(4-maleimidophenoxy)phenyl]ethane, 1, 2-bis[4-(3-maleimidophenoxy)phenyl]ethane, 1,2-bis[4-(4-maleimidophenoxy)phenyl]B Alkane, etc. In addition, as the compound containing at least two or more maleimine groups used in the present invention, a maleidinium group-containing compound represented by the following formula (3) and The maleidinium group-containing compound represented by the formula (4) and the like. The above-mentioned maleimide group-containing compound (A) may be used singly or in combination of two or more kinds.

(式中，η以平均値計爲0〜10。）(where η is 0 to 10 in terms of average enthalpy.)

(式中，η以平均値計爲0〜10。） (Β)酚醛樹脂 本發明中使用的酚醛樹脂（Β)只要是具有酚羥基的化合 物即可，沒有特別限定，優選包括含有至少一個萘環的含 酚羥基化合物。只要滿足上述條件即可，沒有特別限定， 作爲含有至少一個萘環的含酚羥基化合物，具體而言，可 以舉出以下物質。 可以舉出二羥基萘、三羥基萘、四羥基萘等羥基萘類化 合物等。另外，可以舉出使羥基萘類化合物、以及羥基萘 類化合物與酚類化合物的混合物與醛類化合物反應得到的 化合物等。作爲羥基萘類化合物，可以舉出萘酚、二羥基 萘等；作爲酚類化合物，可以舉出苯酚、甲酚、甲苯二酚 等。另外，作爲醛類化合物，可以舉出甲醛、乙醛、苯甲 12 1274771 14873pif.doc 醛等。作爲上述化合物之一例，可以舉出通式（5)表示的化 合物等。(In the formula, η is 0 to 10 in terms of the average enthalpy.) (Phenol) Phenolic resin The phenol resin used in the present invention is not particularly limited as long as it is a compound having a phenolic hydroxyl group, and preferably contains at least one naphthalene. A phenolic hydroxy compound containing a ring. The above conditions are not particularly limited, and specific examples of the phenolic hydroxyl group-containing compound containing at least one naphthalene ring include the following. Examples thereof include hydroxynaphthalene compounds such as dihydroxynaphthalene, trihydroxynaphthalene, and tetrahydroxynaphthalene. Further, a compound obtained by reacting a hydroxynaphthalene compound and a mixture of a hydroxynaphthalene compound and a phenol compound with an aldehyde compound can be given. Examples of the hydroxynaphthalene compound include naphthol and dihydroxynaphthalene; and examples of the phenol compound include phenol, cresol, and toluenediol. Further, examples of the aldehyde compound include formaldehyde, acetaldehyde, and benzophenone 12 1274771 14873 pif. doc aldehyde. An example of the compound is a compound represented by the formula (5).

需要說明的是上述化合物可以利用上述方法製得，作爲 能夠使用的市售品，也可以使用日本化藥株式會社製’ ® 品名·· KAYAHARD NHN等產品。 另外，可以舉出羥基萘類化合物、以及羥基萘類化合物 與酚類化合物的混合物與芳烷基醇衍生物或芳烷基鹵化物 衍生物反應得到的化合物等。作爲芳烷基醇衍生物，可以 舉出對亞二甲苯基二醇、對亞二甲苯基二醇二甲醚等；另 外，作爲芳烷基鹵化物衍生物，可以舉出二氯對二甲苯等。 作爲上述化合物之一例，可以舉出通式（6)表示的化合物等。In addition, the above-mentioned compound can be obtained by the above-mentioned method, and as a commercially available product, a product such as the product name "KAYAHARD NHN" manufactured by Nippon Kayaku Co., Ltd. can be used. Further, examples thereof include a hydroxynaphthalene compound and a compound obtained by reacting a mixture of a hydroxynaphthalene compound and a phenol compound with an aralkyl alcohol derivative or an aralkyl halide derivative. Examples of the aralkyl alcohol derivative include p-xylylene glycol and p-xylylene glycol dimethyl ether; and examples of the aralkyl halide derivative include dichloro-p-xylene. Wait. An example of the compound is a compound represented by the formula (6).

(式中，P爲1或2, η爲1〜10的整數。） 需要說明的是上述化合物可以利用上述方法得到，作爲 可以使用的市售品，也可以使用新日鐵化學株式會社製， 商品名：SN180等產品。 上述酚醛樹脂可以單獨使用，也可以2種或2種以上組 合使用。 (C)環氧樹脂 本發明中使用的環氧樹脂（C)只要是具有環氧基的樹脂 13 1274771 14873pif.doc 即可，沒有特別限定。 本發明使用的環氧樹脂（C)中’優選包括含有至少一個 萘環的環氧化合物。作爲含有至少一個萘環的環氧化合 物，具體而言，可以舉出以下物質。 例如，可以舉出二羥基萘、三羥基萘、四羥基萘等羥基 萘類化合物與表氯醇反應得到的化合物等。需要說明的是 上述化合物可以利用上述方法得到’作爲可以使用的市售 品，可以使用大日本INK化學社製、商品名：EPICLON HP4032 等 。 另外，還可以舉出使萘酚、二羥基萘等羥基萘類化合 物、以及上述羥基萘類化合物與苯酚、甲酚、甲苯二酚等 酚類化合物的混合物與甲醛、乙醛、苯甲醛等醛類化合物 反應的產物進一步與表氯醇反應得到的化合物。作爲上述 化合物的具體例，可以舉出通式（7)表示的化合物等。(In the formula, P is 1 or 2, and η is an integer of 1 to 10.) The above-mentioned compound can be obtained by the above-mentioned method, and it can be used as a commercially available product, and it can also be manufactured by Nippon Steel Chemical Co., Ltd. Product name: SN180 and other products. These phenol resins may be used singly or in combination of two or more kinds. (C) Epoxy resin The epoxy resin (C) used in the present invention is not particularly limited as long as it is an epoxy group-containing resin 13 1274771 14873 pif.doc. The epoxy resin (C) used in the present invention preferably includes an epoxy compound containing at least one naphthalene ring. Specific examples of the epoxide containing at least one naphthalene ring include the following. For example, a compound obtained by reacting a hydroxynaphthalene compound such as dihydroxynaphthalene, trihydroxynaphthalene or tetrahydroxynaphthalene with epichlorohydrin can be mentioned. In addition, the above-mentioned compound can be obtained as a commercially available product by the above-mentioned method, and it can be used by Dainippon Ink Chemical Co., Ltd., trade name: EPICLON HP4032 or the like. Further, a mixture of a hydroxynaphthalene compound such as naphthol or dihydroxynaphthalene, and a phenolic compound such as phenol, cresol or toluene and a aldehyde such as formaldehyde, acetaldehyde or benzaldehyde may be mentioned. The product of the reaction of the compound-like compound is further reacted with epichlorohydrin to obtain a compound. Specific examples of the above compound include a compound represented by the formula (7).

(式中，G爲縮水甘油基，j以平均値計爲0〜10。） 需要說明的是上述化合物可以利用上述方法得到’作爲 可以使用的市售品，可以使用日本化藥株式會社製’商品 名· NC — 7 0 00寺產品。 另外，可以舉出使萘酚、二經基萘等經基萘類化合物以 及上述羥基萘類化合物與苯酚、甲酚、甲苯二酚等酚類化 合物的混合物與芳烷基醇衍生物或芳烷基鹵化物衍生物反 應的產物進一步與表氯醇反應得到的化合物等。作爲上述 14 1274771 14873pif.doc 化合物的具體例，可以舉出通式（8)表示的化合物等。(In the formula, G is a glycidyl group, and j is 0 to 10 in an average enthalpy.) The above-mentioned compound can be obtained as a commercially available product which can be used by the above method, and can be used by Nippon Kayaku Co., Ltd. Product Name · NC — 7 0 00 Temple Products. Further, a mixture of a naphthyl compound such as naphthol or dipyridyl naphthalene and a phenolic compound such as phenol, cresol or toluene with an aralkyl alcohol derivative or an aralkyl group may be mentioned. The product obtained by reacting the product of the base halide derivative with the epichlorohydrin, and the like. Specific examples of the compound of the above-mentioned 14 1274771 14873pif.doc include a compound represented by the formula (8).

(式中’ G爲縮水甘油基，p爲1或2 ’ η表不1〜ι〇的 整數。） 需要說明的是上述化合物可以利用上述方法得到，作胃 可以使用的市售品，可以使用新日鐵化學株式會社製，胃 品名：ESN — 175等產品。上述環氧化合物可以單獨使用， 也可以2種或2種以上組合使用。 另外，本發明的樹脂組成物優選含有液態環氧樹脂作胃 環氧樹脂。液態環氧樹脂沒有特別限定，作爲優選例，$ 以舉出常溫下呈液態的環氧樹脂。作爲具體例，可以舉& 使雙酚A、雙酚F等雙酚與表氯醇反應得到的環氧樹脂以 及其低聚物等。上述液態環氧樹脂可以單獨使用，也柯以 將2種或2種以上組合使用。由於常溫下呈液態的環氧樹 脂分子量較小，在固化時交聯密度增加，可以得到墼_的 樹脂組成物。另外，藉由使其在常溫下呈液態，在製造預 浸體時的乾燥步驟中，能夠賦予樹脂流動性，賦予預浸體 表面平滑性，因此能夠防止皺褶等表面外觀缺陷。 液態環氧樹脂的含量相對於上述樹脂組成物的樹脂成 分（((A)+ (B)+ (C)成分的質量總和）)優選在〜10質量％ 的範圍內。其含量在上述範圍內時，防止表面外觀缺陷的 效果高，樹脂組成物的阻燃性充分，因而是優選採用的。 樹脂組成物 本發明的樹脂組成物含有(A)含有至少2個或2個以上 15 1274771 14873pif.doc 馬來醯亞胺基的化合物，（B)酚醛樹脂，（C)環氧樹脂。 在不影響本發明目的的範圍內，本發明的樹脂組成物還 可以含有上述(A)、（B)以及（C)以外的其他樹脂成分(以下簡 稱爲“其他樹脂成分”）。 (B)酚醛樹脂與（C)環氧樹脂的含量相對於(A)+ (B)+ (C) 成分質量總和，使用（B)與（C)各自的〇H當量、環氧當量計 算得到的萘環質量總和優選爲20質量％或20質量％以 上，更優選爲25質量％或25質量％以上、50質量％或50 質量％以下。 需要說明的是（B)酚醛樹脂中的萘環質量mNap(B)可以 使用下述數學式進行計算。 mNap(B)=((B)的質量）+ ((3)的 〇H 當量）x(l+((B)中的一 個萘環中存在的〇H基數)xi28 另外，（C)環氧樹脂中的萘環質量mNap(C)可以使用下述 數學式進行計算。 mNap(C) = ((C)的質量的環氧當量）x(l +((C)中的 一個萘環中存在的環氧基數）xl28 萘環質量相對於樹脂成分質量總和的比例MNap(total) 可以使用下述數學式進行計算。 MNap(total) = (mNap(B) + mNap(C)) + ((A) + (B) + (C)成分 質量總和） 萘環質量相對於樹脂成分質量總和的比例MNap(total) 爲20質量％或20質量％以上時，樹脂組成物的阻燃性高， 另外，耐濕性也高，而且能夠提高剛性萘環的耐熱性，因 1274771 14873pif.doc 此也能夠提高耐熱性。如果萘環的質量總和不足20質量 %，則難以獲得充分的阻燃性。由於含有萘環的酚醛樹脂 以及環氧樹脂中的萘環含有率以平均値計爲40〜60質量％ 左右，因此萘環的質量總和爲50質量％或50質量％以下 時，樹脂中馬來醯亞胺化合物的含量並不減少，從耐熱性 方面考慮是優選的。 而且，上述樹脂組成物中萘環的含有率MNap(total)與(A) 含馬來醯亞胺基的化合物在(A)+ (B)+ (C)成分中的含有率 Xm的總和爲65質量％或65質量％以上，優選爲70質量 %或70質量％以上。 (A)含馬來醯亞胺基的化合物在（A)+ (B)+ (C)成分中的 含有率可以使用下述數學式求出。(wherein G is a glycidyl group, and p is 1 or 2' η represents an integer of 1 to ι〇.) It is to be noted that the above compound can be obtained by the above method, and can be used as a commercial product which can be used as a stomach. Nippon Steel Chemical Co., Ltd., stomach name: ESN - 175 and other products. These epoxy compounds may be used singly or in combination of two or more kinds. Further, the resin composition of the present invention preferably contains a liquid epoxy resin as a gastric epoxy resin. The liquid epoxy resin is not particularly limited, and a preferred example is an epoxy resin which is liquid at normal temperature. Specific examples thereof include an epoxy resin obtained by reacting bisphenol such as bisphenol A or bisphenol F with epichlorohydrin, and an oligomer thereof. The liquid epoxy resin may be used singly or in combination of two or more kinds. Since the molecular weight of the epoxy resin which is liquid at normal temperature is small, the crosslinking density increases upon curing, and a resin composition of 墼_ can be obtained. Further, by allowing it to be in a liquid state at a normal temperature, it is possible to impart fluidity to the resin and impart smoothness to the surface of the prepreg during the drying step in the production of the prepreg, thereby preventing surface appearance defects such as wrinkles. The content of the liquid epoxy resin is preferably in the range of ～10% by mass based on the resin component of the resin composition (the sum of the masses of the ((A) + (B) + (C) components)). When the content is within the above range, the effect of preventing surface appearance defects is high, and the flame retardancy of the resin composition is sufficient, and therefore it is preferably employed. Resin Composition The resin composition of the present invention contains (A) a compound containing at least 2 or more 15 1274771 14873 pif.doc maleimine groups, (B) a phenol resin, and (C) an epoxy resin. The resin composition of the present invention may further contain other resin components (hereinafter simply referred to as "other resin components") other than the above (A), (B) and (C), insofar as the object of the present invention is not impaired. (B) The content of the phenolic resin and the (C) epoxy resin is calculated from the total mass of the (A) + (B) + (C) component, and is calculated using the 〇H equivalent and the epoxy equivalent of each of (B) and (C). The total mass of the naphthalene ring is preferably 20% by mass or more, more preferably 25% by mass or more, 25% by mass or more, 50% by mass or 50% by mass or less. It is to be noted that the naphthalene ring mass mNap (B) in the (B) phenol resin can be calculated by the following mathematical formula. mNap(B)=(mass of (B))+(〇H equivalent of (3))x(l+(number of 〇H groups present in one naphthalene ring in (B)) xi28 In addition, (C) epoxy resin The naphthalene ring mass mNap(C) can be calculated using the following formula: mNap(C) = ((C) the epoxy equivalent of the mass) x (l + ((C) exists in a naphthalene ring The number of epoxy groups) xl28 The ratio of the mass of the naphthalene ring to the sum of the masses of the resin components MNap(total) can be calculated using the following mathematical formula: MNap(total) = (mNap(B) + mNap(C)) + ((A) (B) + (C) The sum of the masses of the components (C) The ratio of the mass of the naphthalene ring to the total mass of the resin component MNap (total) is 20% by mass or more, and the flame retardancy of the resin composition is high. The moisture resistance is also high, and the heat resistance of the rigid naphthalene ring can be improved, and the heat resistance can be improved by 1274477 14873pif.doc. If the total mass of the naphthalene ring is less than 20% by mass, it is difficult to obtain sufficient flame retardancy. The content of the naphthalene ring in the phenolic resin and the epoxy resin in the ring is about 40 to 60% by mass based on the average enthalpy, so the total mass of the naphthalene ring is 50% by mass or 50%. When the content is less than or equal to 100%, the content of the maleimide compound in the resin is not reduced, and it is preferable from the viewpoint of heat resistance. Further, the content of the naphthalene ring in the above resin composition is MNap (total) and (A) contains Malay. The total content of the content of the quinone imine group compound (X) + (B) + (C) component Xm is 65% by mass or more, preferably 70% by mass or more, or 70% by mass or more. The content of the maleidinium group-containing compound in the (A) + (B) + (C) component can be determined by the following mathematical formula.

Xm=((A)的質量M(A)+ (B)+ (C)成分質量的總和） MNap(total)爲20質量％或20質量％以上，並且 MNap(tQtal：^ Xm的總和爲65質量％或65質量％以上、優 選爲70質量％或70質量％以上時，與萘環的含有率及含 馬來醯亞胺基的化合物單獨爲65質量％或65質量％以上 時相比，樹脂組成物的阻燃性高，並且吸濕性低，吸濕條 件下的耐熱性也高。另一方面，MNap(total)優選爲85質量 %或85質量％以下。MNap(t〇Ul)爲85質量％或85質量％ 以下時，樹脂組成物的脆性低，製成基板材料時，不易發 生斷裂等不良情況，因此是優選的。 含馬來醯亞胺基的化合物（A)的含量相對於（A)+ (B) + (C)成分質量的總和，以含馬來醯亞胺基的化合物(A)中的氮 1274771 14873pif.doc 原子含量計，優選爲3.5質量％或3.5質量％以上、6.5質 量％或6.5質量％以下，更優選爲4.0質量％或4.0質量％ 以上、6.0質量％或6.0質量％以下。樹脂組成物中含馬來 醯亞胺基的化合物(A)的含量在上述範圍內時’由得到的樹 脂組成物製成的基板、積層板等具有充分的阻燃性。需要 說明的是含馬來醯亞胺基的化合物（A)中氮原子含量的最 大値約爲14%左右，因此，酚醛樹脂（B)及環氧樹脂（C)總 和的最大値約爲75質量％左右。 酚醛樹脂(B)與環氧樹脂（C)的配比沒有特別限定’環氧 樹脂（C)中的環氧基數相對於酚醛樹脂（B)中的羥基數優選 爲0.2〜5.0,更優選在0.5〜3.0的範圍內。如果酚醛樹脂(B) 與環氧樹脂（C)的配比在上述範圍內，則樹脂組成物被充分 固化，使積層板具有優良的耐濕性、銲料耐熱性等。 其他樹脂成分 本發明的樹脂組成物除了上述各種成分以外，根據需 要，在不影響阻燃性的範圍內，也可以添加反應性稀釋劑 等成分。 作爲反應性稀釋劑，可以舉出縮水甘油、烯丙基縮水甘 油醚、甲基縮水甘油醚、丁基縮水甘油醚、苯基縮水甘油 醚等通常用於環氧樹脂的反應性稀釋劑；鄰苯二甲酸二烯 丙酯、〇,〇’一二烯丙基雙酚A、雙酚A二烯丙基醚等含有烯 丙基的化合物（上述化合物是通常用於熱固性醯亞胺樹脂 的反應性稀釋劑）。 上述反應性稀釋劑的含量相對於樹脂成分優選在〇·1〜 18 1274771 14873pif.doc 10質量％的範圍內。含量不足0.1質量％時，可能使其作 爲反應性稀釋劑的效果降低；含量大於10質量％時，由於 由樹脂組成物構成的樹脂清漆的黏度顯著降低，因此有時 導致操作性變差。 金屬氫氧化物 優選在本發明的樹脂組成物中進一步添加金屬氫氧化 物。作爲在本發明的樹脂組成物中使用的金屬氫氧化物， 只要是氫氧化鋁、氫氧化鎂、羥基錫酸鋅等具有（011)11的金 屬化合物即可，沒有特別限定，優選氫氧化鋁(ai(oh)3)、 氫氧化鎂(Mg(OH)2)、羥基錫酸鋅（ZnSn(〇H)5)等，更優選氫 氧化銘。 另外，上述金屬氫氧化物中作爲雜質含有的Na20最好 含量較低。Na20含量優選爲不足0.3%，更優選爲C.2%或 0.2%以下，特別優選爲〇〜0.1%。金屬氫氧化物中作爲雜 質含有的Na2〇含量較多時，優選採用進行洗滌的方法、特 開平8 - 32^12號公報等公開的方法等將所含Na2〇含量減 少至不足0·3%後使用。如果金屬氫氧化物中Na2〇的含量 在上述範圍內，則由含有該金屬氫氧化物的耐熱性樹脂組 成物製成的積層板具有特別優良的銲料耐熱性I另外，將 積層板作爲電路基板使用時’不易發生由離子遷移引起的 可靠性劣化。本發明中使用的金屬氫氧化物的粒徑沒有特 別限疋’通？ί使用平均粒徑爲0 · 1〜1 〇以m的物質。上述金 屬氫氧化物可以單獨使用1種，也可以將2種或2種以上 組合使用。 19 1274771 14873pif.doc 另外，優選在上述金屬氫氧化物中使用耦合劑。作爲耦 合劑，可以使用矽烷類、鈦酸鹽類、鋁酸鹽類及锆鋁酸鹽 類等耦合劑。其中，優選矽烷類耦合劑，特別優選具有反 應性官能基的矽烷類耦合劑。 作爲矽烷類耦合劑的具體例，可以舉出乙烯基三甲氧基 石夕院、乙稀基三乙氧基砂院、N—（2—氨基乙基）3 —氨基丙 基甲基二甲氧基矽烷、N—（2—氨基乙基）3 —氨基丙基三甲 氧基矽烷、N-苯基一 r 一氨基丙基三甲氧基矽烷、3-氨 基丙基三乙氧基矽烷、3-苯胺基丙基三甲氧基矽烷、3-環氧丙氧基丙基三甲氧基矽烷、3-環氧丙氧基丙基甲基二 甲氧基矽烷、2—（3,4一乙氧基環己基）乙基三甲氧基矽烷、 3—甲基丙烯醯氧基丙基三甲氧基矽烷、3 —锍基丙基三甲 氧基矽烷等，上述物質可以使用1種、2種或2種以上。優 選將上述矽烷類耦合劑預先藉由吸附或反應固定在金屬氫 氧化物表面。如果使用耦合劑，則能夠提高金屬氫氧化物 與樹脂的黏合性，可以期待提高由樹脂組成物製成的積層 板的機械強度、耐熱性。 在以（A)+(B)+(C)成分質量的總和爲1〇〇質量份時， 金屬氫氧化物的含量爲5〜100質量份，優選爲5〜80質量 份。如果金屬氫氧化物的含量在上述範圍內，則能夠獲得 阻·燃效果，製成清漆時的黏度適當，在基材中的含浸性良 好，操作性優良。另外，金屬氫氧化物的含量超過1〇〇質 量份時（超過樹脂組成物的50wt%時），樹脂組成物的吸水 性高，對吸濕後的銲料耐熱性等產生不良影響。 20 1274771 14873pif.doc 本發明的樹脂組成物實質上不含磷類阻燃劑、鹵素類阻 燃劑’憐類阻燃劑、鹵素類阻燃劑的含量以磷或鹵素換算 爲0.05或0.05以下。需要說明的是日本印刷電路工業界 (JPCA)規定的“無鹵”的定義爲在覆銅積層板中，鹵素含 量爲0.09質量％或0·〇9質量％以下，因此本發明的樹脂組 成物以及形成的積層板符合上述規定。 固化促進劑 本發明的樹脂組成物中還優選含有固化促進劑。作爲固 化促進劑，例如，可以舉出2 —甲基咪唑、2 —乙基一 4 一甲 基咪唑、2—十七烷基咪唑、2一乙基一 4一甲基咪唑基四苯 基硼酸鹽等咪唑類固化促進劑；三乙醇胺、三亞乙基二胺、 N-甲基嗎啉等胺類固化促進劑；四苯基硼酸四苯基鐵、四 苯基硼酸三乙基銨等四苯基硼酸鹽類固化促進劑；1，8-二 氮雜-雙環（5,4,0)十一碳烯一 7及其衍生物等。上述固化促 進劑可以單獨使用，也可以將2種或2種以上組合使用。 上述固化促進劑的含量優選爲能夠得到下述清漆或預 浸體所需要的凝膠化時間的配合量，一般而言，相對於樹 脂成分總量（(A) + (B)+ (C)成分的總量）i〇〇質量份，其含量 在0.005〜5質量份的範圍內。 無機塡充劑 本發明的樹脂組成物中也可以添加無機塡充劑。作爲無 機塡充劑種類的優選例，可以舉出二氧化矽、氧化鋁、氧 化鈦、滑石、鍛燒滑石、高嶺土、雲母、黏土、氮化鋁、 玻璃等。更優選爲二氧化矽、氧化鋁、氧化鈦、滑石，特 21 1274771 14873pif.doc 別優選球狀二氧化矽以及滑石。由於二氧化矽、氧化鋁、 氧化鈦的硬度高，因此少量添加就能夠有助於提高彈性模 數。就形狀而言，使用球狀物質的情況下，在製成樹脂清 漆時，黏度不會急遽升高，隨後的操作性優良，因此是優 選的。特別是滑石爲扁平的形狀時，能夠有助於提高彎曲 彈性模數。無機塡充劑含量相對於樹脂成分總量（(A)+(B) + (C)成分的總量）100質量份，通常優選使用10〜150質量 份。 添加劑 根據不同的用途，也可以在本發明的樹脂組成物中使用 添加劑。作爲添加劑的優選例，可以舉出通常作爲消泡劑、 均染劑、表面張力調整劑使用的添加劑等。作爲具體例， 可以舉出氟類、矽類、丙烯酸類等消泡劑、均染劑。添加 劑的含量相對於樹脂成分總量（(A) + (B) + (C)成分的總 量）100質量份，通常優選使用0.0005〜5質量份。 樹脂組成物的製備方法 本發明的樹脂組成物例如可以如下製備：將含有馬來醯 亞胺基的化合物（A)與酚醛樹脂（B)、環氧樹脂（C)在80〜200 °C下加熱混合〇·1〜10小時，製成均勻的混合物。添加金屬 氫氧化物或無機塡充劑時，可以將上述混合物在常溫下粉 碎，以粉末狀態混合，也可以在下述樹脂清漆中混合上述 金屬氫氧化物或無機塡充劑。 樹脂清漆 本發明的樹脂清漆是將含有馬來醯亞胺基的化合物 22 1274771 14873pif.doc (A)、酚醛樹脂（B)與環氧樹脂（C)溶解在溶劑中而得到的。 作爲樹脂清漆中使用的溶劑，可以舉出乙=旧一乙酸、 丙二醇一甲醚、乙二醇一丁醚、N，N—二甲基二Xm=(sum of mass (M) of (A)+(B)+(C) component) MNap(total) is 20% by mass or more, and MNap(the total of tQtal:^ Xm is 65 When the content is 5% by mass or more, preferably 70% by mass or more, 70% by mass or more, and when the content of the naphthalene ring and the compound containing a maleidino group are 65% by mass or more by mass or more, respectively. The resin composition has high flame retardancy and low hygroscopicity, and high heat resistance under moisture absorbing conditions. On the other hand, MNap (total) is preferably 85 mass% or 85% by mass or less. MNap (t〇Ul) When the content is 85% by mass or less, the resin composition is low in brittleness, and when a substrate material is formed, it is less likely to cause defects such as cracking. Therefore, the content of the compound (A) containing a maleimine group is preferable. The total mass of the component (A) + (B) + (C) is preferably 3.5% by mass or 3.5 mass based on the atomic content of nitrogen 1274771 14873 pif. doc in the compound (A) containing a maleidino group. % or more, 6.5% by mass or 6.5% by mass or less, more preferably 4.0% by mass or more, 4.0% by mass or more, 6.0% by mass or 6.0% by mass When the content of the maleimide group-containing compound (A) in the resin composition is within the above range, the substrate, the laminate, and the like made of the obtained resin composition have sufficient flame retardancy. The maximum enthalpy of the nitrogen atom content in the compound (A) containing a maleimine group is about 14%, and therefore, the maximum enthalpy of the sum of the phenol resin (B) and the epoxy resin (C) is about 75 mass%. The ratio of the phenol resin (B) to the epoxy resin (C) is not particularly limited. The number of epoxy groups in the epoxy resin (C) is preferably 0.2 to 5.0, more preferably the number of hydroxyl groups in the phenol resin (B). In the range of 0.5 to 3.0, if the ratio of the phenol resin (B) to the epoxy resin (C) is within the above range, the resin composition is sufficiently cured to provide the laminate with excellent moisture resistance and solder heat resistance. Other Resin Component The resin composition of the present invention may contain a component such as a reactive diluent, in addition to the above various components, as needed, insofar as the flame retardancy is not affected. Glycerol, allyl glycidol Reactive diluents commonly used in epoxy resins, such as ether, methyl glycidyl ether, butyl glycidyl ether, phenyl glycidyl ether; diallyl phthalate, hydrazine, 〇'-diallyl An allyl-containing compound such as bisphenol A or bisphenol A diallyl ether (the above compound is a reactive diluent generally used for thermosetting quinone imine resins). The content of the above reactive diluent is preferably relative to the resin component. In the range of 10% by mass of 〇·1 to 18 1274771 14873pif.doc, when the content is less than 0.1% by mass, the effect as a reactive diluent may be lowered; when the content is more than 10% by mass, it is composed of a resin composition. The viscosity of the resin varnish is remarkably lowered, and thus the workability is sometimes deteriorated. Metal hydroxide It is preferred to further add a metal hydroxide to the resin composition of the present invention. The metal hydroxide to be used in the resin composition of the present invention is not particularly limited as long as it is a metal compound having (011)11 such as aluminum hydroxide, magnesium hydroxide or zinc hydroxystannate, and aluminum hydroxide is preferred. (ai(oh)3), magnesium hydroxide (Mg(OH)2), zinc hydroxystannate (ZnSn(〇H)5), etc., more preferably hydroxide. Further, the content of Na20 contained as an impurity in the above metal hydroxide is preferably low. The Na20 content is preferably less than 0.3%, more preferably C.2% or 0.2% or less, and particularly preferably 〇~0.1%. When the content of Na 2 ruthenium contained in the metal hydroxide as an impurity is large, it is preferable to reduce the content of Na 2 ruthenium contained to less than 0.3% by a method of washing, a method disclosed in JP-A-8-32-02, or the like. After use. When the content of Na2〇 in the metal hydroxide is within the above range, the laminated board made of the heat resistant resin composition containing the metal hydroxide has particularly excellent solder heat resistance I. Further, the laminated board is used as a circuit board. When used, reliability deterioration due to ion migration is less likely to occur. The particle size of the metal hydroxide used in the present invention is not particularly limited. ί Use a substance with an average particle size of 0 · 1 to 1 〇 m. These metal hydroxides may be used singly or in combination of two or more kinds. 19 1274771 14873pif.doc Further, it is preferred to use a coupling agent in the above metal hydroxide. As the coupling agent, a coupling agent such as a decane, a titanate, an aluminate or a zirconium aluminate can be used. Among them, a decane-based coupling agent is preferable, and a decane-based coupling agent having a reactive functional group is particularly preferable. Specific examples of the decane-based coupling agent include vinyltrimethoxy sylvestre, ethylene triethoxy sand, and N-(2-aminoethyl) 3-aminopropylmethyldimethoxy. Decane, N-(2-aminoethyl) 3-aminopropyltrimethoxydecane, N-phenyl-r-aminopropyltrimethoxydecane, 3-aminopropyltriethoxydecane, 3-aniline Propyltrimethoxydecane, 3-glycidoxypropyltrimethoxydecane, 3-glycidoxypropylmethyldimethoxydecane, 2-(3,4-ethoxycarbonyl) Ethyltrimethoxydecane, 3-methylpropenyloxypropyltrimethoxydecane, 3-mercaptopropyltrimethoxydecane, and the like may be used alone or in combination of two or more. It is preferred that the above decane-based coupling agent is previously fixed to the surface of the metal hydroxide by adsorption or reaction. When a coupling agent is used, the adhesion between the metal hydroxide and the resin can be improved, and the mechanical strength and heat resistance of the laminate made of the resin composition can be expected to be improved. When the total mass of the components (A) + (B) + (C) is 1 part by mass, the content of the metal hydroxide is 5 to 100 parts by mass, preferably 5 to 80 parts by mass. When the content of the metal hydroxide is within the above range, the effect of hindrance and combustion can be obtained, the viscosity at the time of making the varnish is appropriate, the impregnation property in the substrate is good, and the workability is excellent. When the content of the metal hydroxide exceeds 1 part by mass (when it exceeds 50% by weight of the resin composition), the water absorption of the resin composition is high, which adversely affects the heat resistance of the solder after moisture absorption. 20 1274771 14873pif.doc The resin composition of the present invention contains substantially no phosphorus flame retardant, halogen flame retardant, pity flame retardant, halogen flame retardant, and the content of phosphorus or halogen is 0.05 or less. . It is to be noted that the "halogen-free" defined by the Japanese printed circuit industry (JPCA) is defined as a resin composition of the present invention in which the halogen content is 0.09% by mass or less than 9% by mass based on the copper-clad laminate. And the formed laminate is in compliance with the above regulations. Curing accelerator The resin composition of the present invention preferably further contains a curing accelerator. Examples of the curing accelerator include 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-heptadecylimidazole, and 2-ethyl-4-methylimidazolyl tetraphenylborate. An imidazole curing accelerator such as a salt; an amine curing accelerator such as triethanolamine, triethylenediamine or N-methylmorpholine; tetraphenyl iron tetraphenylborate, tetraphenylammonium tetraphenylborate or the like A borate-based curing accelerator; 1,8-diaza-bicyclo(5,4,0)undecene-7 and derivatives thereof. These curing accelerators may be used singly or in combination of two or more kinds. The content of the above-mentioned curing accelerator is preferably a compounding amount of a gelation time required to obtain the following varnish or prepreg, and generally, relative to the total amount of the resin component ((A) + (B) + (C) The total amount of the components is i〇〇 by mass, and the content thereof is in the range of 0.005 to 5 parts by mass. Inorganic chelating agent An inorganic chelating agent may be added to the resin composition of the present invention. Preferable examples of the type of the inorganic ruthenium agent include cerium oxide, aluminum oxide, titanium oxide, talc, calcined talc, kaolin, mica, clay, aluminum nitride, glass, and the like. More preferably, it is cerium oxide, aluminum oxide, titanium oxide, talc, and it is preferable that spherical cerium oxide and talc are preferable. Since the hardness of cerium oxide, aluminum oxide, and titanium oxide is high, a small amount of addition can contribute to an increase in the modulus of elasticity. In the case of using a spherical material in terms of shape, it is preferable that the viscosity is not increased sharply when it is made into a resin varnish, and the subsequent workability is excellent. In particular, when the talc has a flat shape, it can contribute to an increase in the bending elastic modulus. The content of the inorganic chelating agent is usually preferably 10 to 150 parts by mass based on 100 parts by mass of the total amount of the resin component (the total amount of the (A) + (B) + (C) component). Additives Depending on the application, additives may also be used in the resin composition of the present invention. Preferable examples of the additive include an additive which is generally used as an antifoaming agent, a leveling agent, and a surface tension adjusting agent. Specific examples thereof include antifoaming agents such as fluorines, hydrazines, and acrylics, and leveling agents. The content of the additive is usually preferably 0.0005 to 5 parts by mass based on 100 parts by mass of the total amount of the resin component (the total amount of the (A) + (B) + (C) component). Method for Producing Resin Composition The resin composition of the present invention can be prepared, for example, by reacting a compound (A) containing a maleimine group with a phenol resin (B) and an epoxy resin (C) at 80 to 200 ° C. The mixture was heated and mixed for 1 to 10 hours to prepare a homogeneous mixture. When a metal hydroxide or an inorganic chelating agent is added, the above mixture may be pulverized at a normal temperature and mixed in a powder state, or the above metal hydroxide or inorganic cerium may be mixed in the following resin varnish. Resin varnish The resin varnish of the present invention is obtained by dissolving a compound containing a maleimine group 22 1274771 14873 pif.doc (A), a phenol resin (B) and an epoxy resin (C) in a solvent. Examples of the solvent used in the resin varnish include B = old monoacetic acid, propylene glycol monomethyl ether, ethylene glycol monobutyl ether, and N,N-dimethyl two.

避甲醯胺、N，N 一二甲基乙醯胺、二氧雜環己烷、丙酮、甲其—2—吡 略烷酮、二甲基亞砸、甲基乙基酮、甲基異了其^同、環己 烷、2-庚酮等。作爲溶劑，優選沸點較低的溶劑，優選使 用甲基乙基酮、丙酮、二氧雜環己烷或以上述物質爲主成 分的混合物。 在不影響本發明目的的範圍內，本發明的樹脂清漆中也 可以含有上述（A)、（B)及（C)以外的其他樹脂成分。樹脂清 漆中含有馬來醯亞胺基的化合物(A)、酚醛樹脂(B)、環氧樹 脂（C)的含量與上述樹脂組成物相同。 本發明的樹脂清漆中優選含有上述固化促進劑，含 上述樹脂組成物相同。另外，本發明的樹脂清漆中 有上述樹脂組成物中也可含有的“其他樹脂成分，，。樹月旨 清漆中，上述(A)、（B)、（C)以總量計通常含有50〜質里 %，優選在50〜70質量％的範圍內。 樹脂清漆例如可以如下製備：在有機溶劑中加熱混合含 有馬來醯亞胺基的化合物（A)、酚醛樹脂（B)以及瓌氣 (C)、及其他樹脂成分，得到均勻的溶液。加熱混合時的⑽ 度根據有機溶劑的沸點不同而不同，通常爲50〜2〇〇°C ;加 熱混合時間通常爲〇.1〜2〇小時。另外，本發明的樹脂清漆 可以藉由混合溶解上述樹脂組成物與上述溶劑而製得。 預浸體 23 1274771 14873pif.doc 本發明的預浸體是藉由在基材中含浸上述樹脂粗成物 而製成的。本發明的預浸體可以將上述樹脂清漆塗布或含 浸在基材中 '然後乾燥除去溶劑而製成。作爲基材，可以 使用玻璃不織布、玻璃布、碳纖維布、有機纖維布、紙等 可以用於現有預浸體的全部公知基材。將上述樹脂清漆塗 布或含浸在上述基材中後，經過乾燥步驟，製成預浸體， 塗布方法、含浸方法、乾燥方法可以採用現有的公知方法， 沒有特別限定。 就乾燥條件而言，可以根據所使用溶劑的沸點適當決 定，優選使預浸體中的殘留溶劑量爲1質量％或1質量％ 以下的條件。具體而言，可以舉出在140°c〜220°C的範圖 內、滯留時間爲5分鐘〜10分鐘左右的優選條件，在隨後 進行預浸體乾燥的製造步驟中，溫度的優選範圍根據運送 速度不同而發生變化，但是並不限定於此。 積層板 本發明的積層板藉由積層1張或幾張上述預浸體、經熱 壓處理使其加熱固化而製成。製作積層板時的加熱加壓條 件無特別限定，加熱溫度爲100〜300°c、優選爲15〇〜250 °C，壓力爲1·〇〜lOMPa，加熱加壓時間爲10〜300分鐘左 右。 本發明的積層板也包括在上述積層板的兩面使金屬箱 或金屬板積層一體化製成的兩面金屬板。兩面金屬板可以 如下製造：在1張預浸體的一面或兩面上積層金屬范或金 屬板，進行熱壓處理，或在經幾張積層得到的預浸體最外 24 1274771 14873pif.doc 層的兩面上積層金屬箔或金屬板，進行熱壓處理，由此使 預浸體加熱固化’經一體化處理製成上述兩面金屬板。金 屬箔或金屬板沒有特別限定，優選使用銅、鋁、鐵、不鏽 鋼等。加熱固化時的條件爲與上述積層板相同的條件。 而且’本發明的積層板還包括在上述兩面金屬板上形成 了電路的積層板’和交替積層預浸體，在最外層積層金屬 箔或金屬板’經熱壓處理製成的多層積層板。該多層積層 板可以採用在通常的用於多層印刷電路板的積層板的製造 步驟中採用的各種方法，但是並不特別限定於該方法。 (實施例） 下面’基於實施例，更具體地說明本發明，但是本發明 並不限定於下述實施例。 實施例1〜5及比較例1〜2 在80°C下用6小時將表1所示組成（質量份）中（A)〜（C) 及其他樹脂的配合物溶解在燒瓶內的甲基乙基酮：N-甲基 一 2-吡咯烷酮的混合溶劑（混合比爲甲基乙基酮：N-甲基 一 2—吡咯烷酮=4 ·· 1)中，得到樹脂清漆。在由此得到的 樹脂清漆中加入金屬氫氧化物、固化促進劑、無機塡充劑、 添加劑，攪拌均勻，含浸在l〇8g/m2(厚度約l〇〇Vm)的玻 璃布中，在150它下乾燥5分鐘，得到約200 g/m2(厚度約 100// m)的預浸體。將5張該預浸體疊合，再在其上的最外 層上設置18// m的銅箔，在2MPa的壓力下，180〜230°C、 120分鐘的加熱條件下成形，得到厚度爲〇·5〜0.7mm的覆 銅積層板。由此得到的積層板的試驗結果也同樣示於表 25 1274771 14873pif.doc 中。試驗方法如下所示。料，就阻燃性的評價而霄，除 了疊合2張預浸體以外，與上述方法同樣地製成厚度爲0.2 〜0.3mm的覆銅積層板，使用該覆銅積層板進行評價。 (1) 阻燃性·基於UL94 _準的阻燃性試驗方法進行測 定。 (2) 耐濕性：使用高壓鍋，在121。〇、1〇〇%RH、2.1大 氣壓的條件下加濕24小時後，測定重量，以加濕前的重量 爲基準’計算重量變化率，以此爲吸濕率。 (3) 銲料耐熱性··基於JIS C_ 6481，在i2rc、2·；ι大氣 壓、100%RH的條件下對試驗片進行3小時吸水處理後， 在任意溫度的銲料浴中熱流60秒，以銅箔部分不發生膨脹 的最高溫度爲耐熱溫度。 實施例及比較例中使用以下原料： (A) 含有馬來醯亞胺基的化合物 BMI — S(商品名’氮原子含量：約8%，分子量：358， 三井化學（株)社製） BMI- MP(商品名，氮原子含量：約1〇%，分子量：268， 三井化學（株）社製） (B) 酚醛樹脂 萘酚芳烷基樹脂，SN180(商品名，OH當量190，一個 萘環中的OH基數：1，新日鐵化學（株)社製） 萘酚芳烷基樹脂，SN485(商品名，OH當量215，一個 察環中的OH基數：1，新日鐡化學（株/社製） (C) 環氧樹脂 26 1274771 14873pif.doc 萘型環氧樹脂、EPICLON HP4032(商品名，環氧當量 150, 一個萘環中的環氧基數：2,大日本INK化學工業（株） 社製） 萘酚芳烷基型環氧樹脂、ESN175(商品名，環氧當量 270，一個萘環中的環氧基數：1，新日鐵化學（株)社製） 二羥基萘芳烷基型環氧樹脂、ESN375(商品名，環氧當 量170，一個萘環中的環氧基數：2，新日鐵化學（株)社製） 液態雙酚A型環氧樹脂、EPIKOTE828EL(商品名，環 氧當量190，不含有萘環，Japan Epoxy Resins(株)社製） 其他樹脂成分： 反應稀釋劑：烯丙基縮水甘油醚（Ep1〇l A(商品名），日 本油脂（株)社製） 固化促進劑：2 —乙基—4 —甲基咪唑（2E4MZ(商品名）， 四國化成工業（株)社製） 金屬氫氧化物： 氫氧化鋁，HS— 330(商品名，平均粒徑·· 7// m，Na2〇 量：0.04%，昭和電工(株)社製） 氫氧化鋁，CL— 303(商品名，中心粒徑：2.5// m，Na2〇 量：0.21%，住友化學工業（株)社製） 無機塡充劑： 球狀二氧化矽，SO — C2(商品名，平均粒徑：0.5// m， 龍森（株)社製） 添加齊彳（均染劑）：FTX218(商品名，Neos(株)社製） 27 Ι27477ΐ3ρίΜο° 表1 成分名及試驗項目 實施例 比較例 1 2 3 4 5 1 2 (A)馬來醯亞胺 •BMI-S 55 55 50 45 50 50 •BMI-MP 50 (B)酚醛樹脂 •SN485 16 16 18 11 16 16 •SN180 12 (C)環氧樹脂 •HP4032 27 13 •ESN 175 •ESN375 29 27 31 37 •EPDCOTE828EL 2 2 2 16 29 反應性稀釋劑 5 5 5 5 5 固化促進劑 0.05 0.05 0.05 0.05 0.05 金屬氫氧化物 •HS-330 25 35 80 133 •CL303 50 13 無機塡充劑 25 20 添加劑 0.005 0.005 Mnap(total) 23% 22% 22% 20% 24% 15% 10% Mnap(t〇tal)+Xm 78% 77% 72% 70% 69% 65% 60% 氮％ 4.4 4.4 5 4 3.6 4 4 阻燃性(〇.2mm) V-1 V-0 V-0 V-1 V-0 V -2out V-0 加濕銲料耐熱性.。C 280 280 280 280 280 260 <260 吸濕率 1.0% 1.0% 1.0% 1.1% 0.9% 1.5% 2.4% 與實施例相比，比較例1的Mnap(total)不足20%，阻燃 性不充分；另外，由於比較例2中氫氧化物的添加量多， 因此雖然阻燃性不充分，但是樹脂組成物中萘環的質量總 和未達到20質量％或20質量％以上，另外，由於 Mnap(total)+Xm也不足65%，因此與實施例相比，加濕後的 銲料耐熱性降低，吸濕率也高。 28 iif.doc 工業實用件 由於能夠在不含有鹵素化合物、磷化合物的前提下得到 阻燃性，因此作爲電子部件等中使用的印刷電路板材料， 可以作爲環境負荷小（不含有能夠對環境產生不良影響的 化合物）的材料使用。另外，由於耐濕性、耐濕熱性優良， 因此可以在使用無鉛銲料的過程中使用，其結果爲即使形 成銲料封裝後的電子部件整體，環境負荷也較小。 【圖式簡單說明】 Μ j\ \\ 【主要元件符號說明】Avoiding formazan, N,N-dimethylammoniumamine, dioxane, acetone, methyl 2-pyrrolidone, dimethyl azine, methyl ethyl ketone, methyl It is the same, cyclohexane, 2-heptanone and the like. As the solvent, a solvent having a relatively low boiling point is preferred, and methyl ethyl ketone, acetone, dioxane or a mixture containing the above-mentioned materials as a main component is preferably used. The resin varnish of the present invention may contain other resin components other than the above (A), (B) and (C) insofar as it does not impair the object of the present invention. The content of the compound (A), the phenol resin (B), and the epoxy resin (C) containing a maleidino group in the resin varnish is the same as that of the above resin composition. The resin varnish of the present invention preferably contains the above-mentioned curing accelerator, and the resin composition is the same. Further, in the resin varnish of the present invention, the "other resin component" which may be contained in the above resin composition may be contained. In the varnish, the above (A), (B), and (C) usually contain 50 in total. The % by mass is preferably in the range of 50 to 70% by mass. The resin varnish can be prepared, for example, by heating and mixing a compound (A) containing a maleimine group, a phenol resin (B), and a helium gas in an organic solvent. (C), and other resin components, to obtain a uniform solution. The degree of (10) heating and mixing varies depending on the boiling point of the organic solvent, usually 50 to 2 ° C; the heating mixing time is usually 〇.1~2〇 Further, the resin varnish of the present invention can be obtained by mixing and dissolving the above resin composition and the above solvent. Prepreg 23 1274771 14873pif.doc The prepreg of the present invention is obtained by impregnating the substrate with the above resin The prepreg of the present invention can be prepared by coating or impregnating the above resin varnish in a substrate and then drying and removing the solvent. As the substrate, glass non-woven fabric, glass cloth, carbon fiber cloth, organic can be used. Weaving cloth, paper, etc. can be used for all known substrates of the existing prepreg. After the above resin varnish is coated or impregnated in the above-mentioned base material, it is subjected to a drying step to prepare a prepreg, a coating method, an impregnation method, and a drying method. The conventionally known method can be used, and it is not particularly limited. The drying conditions can be appropriately determined depending on the boiling point of the solvent to be used, and the amount of the residual solvent in the prepreg is preferably 1% by mass or less. The preferred conditions are in the range of 140 ° c to 220 ° C and the residence time is about 5 minutes to 10 minutes. In the subsequent manufacturing step of prepreg drying, the preferred range of temperature is based on the transport. The speed varies depending on the speed, but is not limited thereto. The laminated board of the present invention is produced by laminating one or a plurality of the above-mentioned prepregs and heat-treating them by heat pressing. The heating and pressing conditions are not particularly limited, and the heating temperature is 100 to 300 ° C, preferably 15 Torr to 250 ° C, the pressure is 1 〇 to 10 MPa, and the heating and pressing time is about 10 to 300 minutes. The laminated board of the present invention also includes a double-sided metal plate formed by integrally laminating a metal case or a metal plate on both sides of the laminated board. The double-sided metal plate can be manufactured by laminating a metal on one or both sides of a prepreg. Or a metal plate, which is subjected to hot pressing treatment, or a metal foil or a metal plate is laminated on both sides of the outermost 24 1274771 14873pif.doc layer of the prepreg obtained by several layers, and is subjected to hot pressing treatment, thereby heating the prepreg The double-sided metal sheet is formed by the integrated treatment. The metal foil or the metal plate is not particularly limited, and copper, aluminum, iron, stainless steel, or the like is preferably used. The conditions at the time of heat curing are the same conditions as those of the above laminated sheet. The laminated board of the invention further comprises a laminated board in which an electric circuit is formed on the above-mentioned double-sided metal plate and an alternate laminated prepreg, and a multi-layer laminated board in which the outermost layer of the metal foil or the metal plate is subjected to hot pressing treatment. The multilayer laminated board can employ various methods employed in the usual manufacturing steps of the laminated board for a multilayer printed circuit board, but is not particularly limited to the method. (Embodiment) Hereinafter, the present invention will be described more specifically based on the examples, but the present invention is not limited to the following examples. Examples 1 to 5 and Comparative Examples 1 to 2 The methyl group in the flask was dissolved in a composition of (A) to (C) and other resins in the composition (parts by mass) shown in Table 1 at 80 ° C for 6 hours. Ethyl ketone: a mixed solvent of N-methyl- 2-pyrrolidone (mixing ratio of methyl ethyl ketone: N-methyl-2-pyrrolidone = 4 ··1), and a resin varnish was obtained. A metal hydroxide, a curing accelerator, an inorganic chelating agent, and an additive are added to the resin varnish thus obtained, and the mixture is uniformly stirred, and impregnated in a glass cloth of 10 8 g/m 2 (thickness of about 1 〇〇Vm) at 150 It was dried for 5 minutes to give a prepreg of about 200 g/m2 (thickness about 100//m). Five sheets of the prepreg were laminated, and then 18//m copper foil was placed on the outermost layer, and formed under the pressure of 2 MPa at 180 to 230 ° C for 120 minutes to obtain a thickness of 〇·5~0.7mm copper clad laminate. The test results of the thus obtained laminate are also shown in Table 25 1274771 14873pif.doc. The test method is as follows. In the evaluation of the flame retardancy, a copper-clad laminate having a thickness of 0.2 to 0.3 mm was produced in the same manner as the above method except that two sheets of the prepreg were superposed, and the copper-clad laminate was used for evaluation. (1) Flame retardancy • Measured according to the UL94 _ standard flame retardancy test method. (2) Moisture resistance: Use a pressure cooker at 121. After humidification for 24 hours under conditions of 〇, 1〇〇% RH, and 2.1 atm, the weight was measured, and the weight change rate was calculated based on the weight before humidification as the moisture absorption rate. (3) Solder heat resistance · Based on JIS C_ 6481, the test piece was subjected to water absorption treatment for 3 hours under conditions of i2rc, 2·; ι atmospheric pressure and 100% RH, and then heat flow was performed for 60 seconds in a solder bath of any temperature to The highest temperature at which the copper foil portion does not swell is the heat resistant temperature. In the examples and the comparative examples, the following materials were used: (A) Compound BMI-S containing a maleimide group (trade name 'nitrogen atom content: about 8%, molecular weight: 358, manufactured by Mitsui Chemicals Co., Ltd.) BMI - MP (trade name, nitrogen atom content: about 1%, molecular weight: 268, manufactured by Mitsui Chemicals Co., Ltd.) (B) Phenolic resin naphthol aralkyl resin, SN180 (trade name, OH equivalent 190, one naphthalene) The number of OH groups in the ring: 1, Nippon Steel Chemical Co., Ltd.) Naphthol aralkyl resin, SN485 (trade name, OH equivalent 215, OH group number in one ring: 1, Shin Nikko Chemical Co., Ltd. /Certificate) (C) Epoxy resin 26 1274771 14873pif.doc Naphthalene epoxy resin, EPICLON HP4032 (trade name, epoxy equivalent 150, number of epoxy groups in a naphthalene ring: 2, Dainippon INK Chemical Industry Co., Ltd. ) Naphthol aralkyl type epoxy resin, ESN 175 (trade name, epoxy equivalent: 270, number of epoxy groups in one naphthalene ring: 1, manufactured by Nippon Steel Chemical Co., Ltd.) Base type epoxy resin, ESN375 (trade name, epoxy equivalent 170, number of epoxy groups in a naphthalene ring: 2, Nippon Steel Chemical Co., Ltd. ))) Liquid bisphenol A type epoxy resin, EPIKOTE 828EL (trade name, epoxy equivalent 190, no naphthalene ring, manufactured by Japan Epoxy Resins Co., Ltd.) Other resin components: Reaction diluent: allyl shrinkage Glyceryl ether (Ep1〇l A (trade name), manufactured by Nippon Oil & Fat Co., Ltd.) Curing accelerator: 2-ethyl-4-methylimidazole (2E4MZ (trade name), manufactured by Shikoku Chemicals Co., Ltd. Metal hydroxide: aluminum hydroxide, HS-330 (trade name, average particle size··7//m, Na2〇: 0.04%, manufactured by Showa Denko Co., Ltd.) Aluminum hydroxide, CL-303 ( Product name, center particle size: 2.5// m, Na2 〇 quantity: 0.21%, manufactured by Sumitomo Chemical Co., Ltd.) Inorganic sputum filling: Spherical cerium oxide, SO - C2 (trade name, average particle size: 0.5//m, manufactured by Ronsen Co., Ltd.) Adding 彳 (smoothing agent): FTX218 (trade name, manufactured by Neos Co., Ltd.) 27 Ι27477ΐ3ρίΜο° Table 1 Component name and test item Example Comparative example 1 2 3 4 5 1 2 (A) Maleimide • BMI-S 55 55 50 45 50 50 • BMI-MP 50 (B) Phenolic Resin • SN485 16 16 18 11 16 16 • SN180 12 (C) Epoxy Resin • HP4032 27 13 • ESN 175 • ESN375 29 27 31 37 • EPDCOTE 828EL 2 2 2 16 29 Reactive Diluent 5 5 5 5 5 Curing Accelerator 0.05 0.05 0.05 0.05 0.05 Metal Hydroxide • HS-330 25 35 80 133 • CL303 50 13 Inorganic chelating agent 25 20 Additive 0.005 0.005 Mnap(total) 23% 22% 22% 20% 24% 15% 10% Mnap(t〇tal)+Xm 78% 77% 72% 70% 69% 65% 60% Nitrogen% 4.4 4.4 5 4 3.6 4 4 Flame retardancy (〇.2mm) V-1 V-0 V-0 V-1 V-0 V -2out V-0 Humidifying solder heat resistance. C 280 280 280 280 280 260 <260 moisture absorption rate 1.0% 1.0% 1.0% 1.1% 0.9% 1.5% 2.4% Compared with the examples, the Mnap (total) of Comparative Example 1 was less than 20%, and the flame retardancy was insufficient. In addition, since the amount of the hydroxide added in Comparative Example 2 is large, the flame retardancy is insufficient, but the total mass of the naphthalene ring in the resin composition does not reach 20% by mass or more, and in addition, due to Mnap ( Since the total) + Xm is also less than 65%, the solder after humidification has lower heat resistance and higher moisture absorption rate than in the examples. 28 iif.doc Industrially available parts can be used as a printed circuit board material for electronic components and the like because they can be flame-retardant without containing a halogen compound or a phosphorus compound. The material of the adversely affected compound). Further, since it is excellent in moisture resistance and moist heat resistance, it can be used in the process of using lead-free solder, and as a result, even if the entire electronic component after solder encapsulation is formed, the environmental load is small. [Simple description of the diagram] Μ j\ \\ [Description of main component symbols]

Claims (1)

1274771 14873pif.doc 修正Η期分5〜年3 Η 4丨| : 1 1 ^ m j I 各 L·—. _尤 •«••Η·» 一.-ο·—.»··*·»»·»·一.. ^ R 爲第93 13020丨號中文專利範圍無劃線修正本 十、申請專利範圍： 1· 一種樹脂組成物，含有 (A) 含有至少2個或2個以上馬來醯亞胺基的化合物， (B) 酚醛樹脂， (C) 環氧樹脂， 其特徵爲，使用（B)和（C)各自的OH當量、環氧當量計 算的萘環質量總和相對於（A)+(B)+(C)成分質量總和爲20 質量％或20質量％以上，且（A)的含量相對於（A)+ (B)+ (C) 成分質量總和，以馬來醯亞胺環中含有的氮原子含量計爲 3·5質量％或3.5質量％以上，並且（A)成分相對於（A)+(B) + (C)成分總質量的含有率與該萘環含有率的總和爲65質 量％或65質量％以上。 2·如申請專利範圍第1項所述的樹脂組成物，其特徵 爲，該樹脂組成物中還含有金屬氫氧化物。 3·—種預浸體，其特徵爲，所述預浸體是藉由使申請專 利範圍第1項所述的樹脂組成物含浸在基材中而得到的。 4. 一種積層板，其特徵爲，所述積層板是藉由將由1張 或幾張申請專利範圍第3項所述的預浸體積層而成的材料 加熱固化而得到的。 5. —種積層板，其特徵爲，該積層板含有由申請專利_ 圍第】項所述的樹脂組成物得到的樹脂作爲絕緣層。 301274771 14873pif.doc Revision period 5 to 3 years Η 4丨| : 1 1 ^ mj I Each L·—. _尤•«••Η·» 一.-ο·—.»··*·»» ···一.. ^ R is the 93rd Japanese Patent No. 93 13020. No slash correction. Tenth, the scope of application: 1. A resin composition containing (A) containing at least 2 or more Malay 醯An imine based compound, (B) a phenolic resin, (C) an epoxy resin characterized by the sum of the naphthalene ring masses calculated using the respective OH equivalents and epoxy equivalents of (B) and (C) relative to (A) +(B)+(C) The sum of the masses of the components is 20% by mass or more, and the content of (A) is the sum of the masses of (A)+(B)+(C) components, and the maleimide is The content of the nitrogen atom contained in the ring is 3.5% by mass or more and 3.5% by mass or more, and the content of the component (A) relative to the total mass of the (A) + (B) + (C) component and the naphthalene ring content rate The sum of them is 65 mass% or more. 2. The resin composition according to claim 1, wherein the resin composition further contains a metal hydroxide. A prepreg obtained by impregnating a resin composition according to claim 1 of the patent application with a base material. A laminated board obtained by heat-curing a material obtained by one or a plurality of prepreg layers according to item 3 of the patent application. A laminated board characterized in that the laminated board contains a resin obtained from the resin composition described in the patent application, as an insulating layer. 30
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